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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY · 2018 ·Vol. 18 ·期 12 ·8085-8093 · IF 1.354

A Novel Method of Synthesis of Fluorescent Carbon Dots for Supersensitive and Selective Detection of Cancer Markers

Qi Jianrong,Hu Meixin,Li Hongxia,Jing Ruan,Shen Guangxia

Due to the dual role as an electron acceptor and an electron donor in solution, carbon dots (Cdots) have broad applications in environmental analysis, biological detection, and biosensors. Herein, we report a facile-green strategy for a large-scale synthesis of fluorescent N, P-doped carbon dots (N, P-Cdots) with an absolute quantum yield of 66.08% by a simple one-step thermal decomposition. Glucose was selected as a carbon precursor and tryptophan (Trp) as an N-doping and passivation reagent. Organic polar solvents with a high boiling point, i.e., ethylene glycol and glycerol, were used as the reaction medium, and phosphoric acid was employed as a P source and oxidation accelerator. It is shown that the emission wavelength of the N, P-Cdots can be tuned by adjusting the reaction conditions, such as mass ratio, heating time, temperature, and medium, without further passivation. Finally, advantage was taken of the superior fluorescent characteristics of N, P-Cdots to detect selectively and with high sensitivity a cancer marker, carcinoembryonic antigen (CEA), based on the fluorescent quenching mechanism. Additionally, CEA was also detected in human serum samples with high efficiency and RSD, further confirming that the proposed method has a good consistency and stability for supersensitive fluorimetric detection of cancer markers.

研究领域: 分析化学 · 生物医学 · 材料科学
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Micromachines · 2018 ·Vol. 9 ·期 9 ·470 · IF 2.222

Measurement of Carcinoembryonic Antigen in Clinical Serum Samples Using a Centrifugal Microfluidic Device

Zhigang Gao,Zongzheng Chen,Jiu Deng,Xiaorui Li,Yueyang Qu,Lingling Xu,Yong Luo,Yao Lu,Tingjiao Liu,Weijie Zhao,Bingcheng Lin

Carcinoembryonic antigen (CEA) is a broad-spectrum tumor marker used in clinical applications. The primarily clinical method for measuring CEA is based on chemiluminescence in serum during enzyme-linked immunosorbent assays (ELISA) in 96-well plates. However, this multi-step process requires large and expensive instruments, and takes a long time. In this study, a high-throughput centrifugal microfluidic device was developed for detecting CEA in serum without the need for cumbersome washing steps normally used in immunoreactions. This centrifugal microdevice contains 14 identical pencil-like units, and the CEA molecules are separated from the bulk serum for subsequent immunofluorescence detection using density gradient centrifugation in each unit simultaneously. To determine the optimal conditions for CEA detection in serum, the effects of the density of the medium, rotation speed, and spin duration were investigated. The measured values from 34 clinical serum samples using this high-throughput centrifugal microfluidic device showed good agreement with the known values (average relative error = 9.22%). These results indicate that the high-throughput centrifugal microfluidic device could provide an alternative approach for replacing the classical method for CEA detection in clinical serum samples.Keywords:centrifugal microfluidic device;CEA detection;density medium;fluorescent chemiluminescence

研究领域: 生物医学工程 · 临床检验学
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BIOELECTROCHEMISTRY · 2021 · IF 5.373

Ti3C2 MXene anchors CuAu-LDH multifunctional two-dimensional nanomaterials for dual-mode detection of CEA in electrochemical immunosensors

Mengmeng Zhang,Lisha Mei,Li Zhang,Xiao Wang,Xiaochen Liao,Xiuwen Qiao,Chenglin Hong

Electrochemical immunoassays are commonly used to detect biomarkers and Ti 3 C 2 MXene anchored CuAu-LDH two-dimensional hydroxide heterojunctions for dual-mode electrochemical immunosensors were fabricated in this work. Layered double hydroxides have a large surface area, high chemical stability, tunable metal composition and interchangeable anions, however, the insulating nature of LDH further limits its catalytic performance. For this reason, Ti 3 C 2 Mxenes were introduced to improve this problem. 2D layers of Ti 3 C 2 Mxenes with large specific surface area and excellent conductivity have been well proven and widely used. And the surface of Ti 3 C 2 Mxenes (due to the presence of abundant surface functional groups), will facilitate the anchoring of metal ions and the nucleation of LDH. In addition, its excellent electrical conductivity will facilitate the electron transfer between Cu 2+ and Cu + . The immunosensor not only showed a heavy square wave voltammetry (SWV) signal. It also exhibited high electrocatalytic activity for H 2 O 2 redox reactions and improves the sensitivity of the Ampere Current (i-t) detection. The CEA immunosensor developed in this study showed a wide linear response (0.0001–80 ng/mL) and the lowest detection limits (SWV: 33.6 fg/mL and i-t: 45.4 fg/mL S/N = 3). The results confirmed the excellent analytical capability of the immunosensor.

CAS / MDL: 16961-25-4
研究领域: 生物医学工程 · 分析化学 · 材料科学
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MICROCHIMICA ACTA · 2024 ·Vol. 191 ·期 5 ·1-12 · IF 5.3

Hydrangea-like TiO2/Bi2MoO6 porous nanoflowers triggering highly sensitive electrochemical immunosensing to tumor marker

Ouyang Ruizhuo,Feng Meina,Liu Jinyao,Wang Caihong,Wang Zhongmin,Hu Xin,Miao Yuqing,Zhou Shuang

Rapid and sensitive detection of carcinoembryonic antigen (CEA) is of great significance for cancer patients. Here, molybdenum (Mo) was doped into bismuth oxide (Bi 2 O 3 ) by one-pot hydrothermal method forming porous tremella Bi 2 MoO 6 nanocomposites with a larger specific surface area than the spherical structure. Then, a new kind of hydrangea-like TiO 2 /Bi 2 MoO 6 porous nanoflowers (NFs) was prepared by doping titanium into Bi 2 MoO 6 , where titanium dioxide (TiO 2 ) grew in situ on the surface of Bi 2 MoO 6 nanoparticles (NPs). The hydrangea-like structure provides larger specific surface area, higher electron transfer ability and biocompatibility as well as more active sites conducive to the attachment of anti-carcinoembryonic antigen (anti-CEA) to TiO 2 /Bi 2 MoO 6 NFs. A novel label-free electrochemical immunosensor was then constructed for the quantitative detection of CEA using TiO 2 /Bi 2 MoO 6 NFs as sensing platform, showing a good linear relationship with CEA in the concentration range 1.0 pg/mL ~ 1.0 mg/mL and a detection limit of 0.125 pg/mL (S/N = 3). The results achieved with the designed immunosensor are comparable with many existing immunosensors used for the detection of CEA in real samples. Graphical abstract

研究领域: 生物医学工程 · 分析化学 · 材料科学
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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

Temperature Platform Constructed Using a Cu2O–Cu31S16 Photothermal Conversion System for the Simple Quantitative Analysis of Tumor Markers

Chaoyun Ma,Chulei Zhao,Chenglin Hong,Li Zhang,Siyu Chen,Yu Qi

The quantitative detection of carcinoembryonic antigen (CEA) indicators is a critical step in the early clinical diagnosis of cancer because CEA is closely related to the development of cancer. However, the most commonly used methods for CEA detection mainly involve comparing or measuring the color depth of colored substance solutions, which is not highly accurate, particularly when a second colored substance is present in the solution to be evaluated. Herein, we rationalized the design of a photothermal probe based on calcium carbonate (CaCO3) as a protective shell (Cu2O@CaCO3) for cuprous oxide (Cu2O) nanoparticles to prevent Cu2O oxidation and hyaluronic acid (HA) to confer material biocompatibility (Cu2O@CaCO3@HA). Cu2O can be specifically activated by hydrogen sulfide (H2S), transformed into Cu31S16 nanoparticles and display significant photothermal properties that can be visualized for bioanalysis by simply recording the temperature signal with a thermal imager. In addition, the presence of redox pairs can provide further electrochemically assisted validation of the temperature identification system. Given the portable, economical, and sensitive biosensing, we anticipate that future activatable nanoprobes may be used to assist in early cancer diagnosis and screening.

研究领域: 医学诊断 · 纳米生物技术 · 癌症研究
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ANALYTICAL CHEMISTRY · 2017 · IF 6.32

Near-Infrared-to-Ultraviolet Light-Mediated Photoelectrochemical Aptasensing Platform for Cancer Biomarker Based on Core–Shell NaYF4:Yb,Tm@TiO2 Upconversion Microrods

Zhenli Qiu,Jian Shu,Dianping Tang

Titanium dioxide (TiO2; as a potential photosensitizer) has good photocurrent performance and chemical stability but often exhibits low utilization efficiency under ultraviolet (UV) region excitation. Herein, we devised a near-infrared light-to-UV light-mediated photoelectrochemical (PEC) aptasensing platform for the sensitive detection of carcinoembryonic antigen (CEA) based on core–shell NaYF4:Yb,Tm@TiO2 upconversion microrods by coupling with target-triggered rolling circle amplification (RCA). The upconversion microrods synthesized through the hydrothermal reaction could act as a photosensing platform to convert the near-infrared (near-IR) excitation into UV emission for generation of photoinduced electrons. The target analyte was determined on a functional magnetic bead by using the corresponding aptamers with a sandwich-type assay format. Upon target CEA introduction, a complex was first formed between capture aptamer-1-conjugated magnetic bead (Apt1-MB) and aptamer-2-primer DNA (Apt2-pDNA). Thereafter, the carried primer DNA by the aptamer-2 paired with linear padlock DNA to trigger the RCA reaction. The guanine (G)-rich product by RCA reaction was cleaved by exonuclease I and exonuclease III (Exos I/III), thereby resulting in the formation of numerous individual guanine bases to enhance the photocurrent of core–shell NaYF4:Yb,Tm@TiO2 upconversion microrods under near-IR illumination (980 nm). Under optimal conditions, the near-IR light-mediated PEC aptasensing system could exhibit good photoelectrochemical response toward target CEA and allowed for the detection of target CEA as low as 3.6 pg mL–1. High reproducibility and good accuracy were achieved for analysis of human serum specimens. Importantly, the near-IR-activated PEC aptasensing scheme provides a promising platform for ultrasensitive detection of other biomolecules.

研究领域: 生物医学工程 · 分析化学 · 癌症诊断
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PROCESS BIOCHEMISTRY · 2019 · IF 2.883

Colorimetric and photothermal dual-mode immunoassay for tumour marker detection based on a Ag2CO3@Ag nanocomposite

Bing Zhang,Yejing Jia,Jing Wang,Honghong Chang,Zhihuan Zhao,Yan Cheng

Under the limitations of advanced instruments and professional operations, straightforward readouts play an increasingly vital role in immunoassays. Herein, a Ag 2 CO 3 @Ag nanocomposite-mediated colorimetric and photothermal immunoassay was developed to detect carcinoembryonic antigen (CEA). The Ag 2 CO 3 @Ag nanocomposites could oxidize 3,3’,5,5’-tetramethylbenzidine to form blue oxidation products (TMB ox ) due to the acidic dissolution of Ag 2 CO 3 under acidic conditions. TMB ox presented a strong photothermal effect driven by a near-infrared (NIR) laser. Therefore, TMB ox could act as a photothermal probe to convert immunoassay signals into thermal signals. The Ag 2 CO 3 @Ag nanocomposite was characterized by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and X-ray powder diffraction (XRD). Then, a sandwich-type immunoassay was built on the surface of a magnetic bead, and CEA was quantified using a common thermometer based on the photothermal effect. Under optimal conditions, the temperature increased with increase of CEA concentrations in the range of 0.1 ng/mL–5 ng/mL. More importantly, this system exhibited high selectivity, good repeatability and outstanding stability.

研究领域: 生物化学 · 医学诊断 · 纳米技术
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BULLETIN OF THE KOREAN CHEMICAL SOCIETY · 2017 ·Vol. 38 ·期 10 ·1143-1148 · IF 0.602

An Aptamer-based Self-Catalytic Colorimetric Assay for Carcinoembryonic Antigen

Mingjing Zou,Shuyu Wang

We report a visualization assay for carcinoembryonic antigen (CEA). The assay was prepared based on target-specific recognition, aptamer-based DNAzyme self-catalysis, and colorimetric reaction. Aptamer of CEA was gathered at the surface of magnetic beads for sandwiched co-conjugate when CEA was added. The second aptamer (Apt2) on the beads was folded into G-quadruplex by KCl to make G-quadruplex-hemin DNAzyme with hemin. Apt2-based DNAzyme catalyzed H 2 O 2 -mediated oxidation of 3,3′,5,5′-tetramethylbenzidine, resulting in color changes and significant increase in absorption intensity at 450 nm (Δ A 450nm ). Yellow products can be observed with naked eyes when over 1.0 ng/mL CEA was added and there was a linear correlation between Δ A 450 nm and CEA concentrations in the range of 0.1–8.0 ng/mL with the detection limit of 0.06 ng/mL. The proposed method was then used to determine CEA in human serum from healthy people and tumor patients, revealing a correlation with data from the electrochemiluminescent immunoassay. Owing to its simplicity, selectivity, and low-cost, this method is a promising candidate for detecting CEA and clinical diagnosis of cancer.

CAS / MDL: 70024-90-7
研究领域: 生物化学 · 分析化学 · 分子生物学 · 临床诊断
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2023 · IF 5.2

Biocompatible protein nanogels as robust signal labels for persistent chemiluminescence immunoassays

Yanan Lou,Tong Jiang,Jiangle Yi,Xiang Ren,Xueying Wang,Dawei Fan,Hongmin Ma,Qin Wei

Nanostructured materials with elegant properties have promising potentials in chemiluminescence (CL) immunoassay . However, the robust preparation of such nanomaterials is still challenging. In this work, biocompatible and easily prepared gelatin/horseradish peroxidase (Gel/HRP) nanogels were exploited as signal labels for chemiluminescence immunoassays. The catalytic property of HRP was well retained and the stability was improved after the incorporation into nanogels. The prepared protein nanogels show enhanced and glow-type luminescence behaviors in luminol-H 2 O 2 CL system. Persistent and sensitive CL immunoassay for CEA were constructed using Gel/HRP nanogels as signal labels. A wide linear response range from 0.01 to 100 ng/mL was obtained with the limit of detection was 3.39 pg/mL (S/N = 3).

CAS / MDL: 9048-46-8 6902-77-8
研究领域: 生物材料学 · 分析化学 · 医学检测
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SENSORS AND ACTUATORS B-CHEMICAL · 2021 · IF 7.46

An immunosensor using functionalized Cu2O/Pt NPs as the signal probe for rapid and highly sensitive CEA detection with colorimetry and electrochemistry dual modes

Xiao Wang,Xiaochen Liao,Lisha Mei,Mengmeng Zhang,Siyu Chen,Xiuwen Qiao,Chenglin Hong

Compared with single response systems, dual-mode sensors have attracted much attention due to their high accuracy and high sensitivity. In this work, we successfully combined the high sensitivity of the electrochemical analysis method with the simplicity and rapidity of colorimetric analysis technology to construct a device that can accurately and quickly detect CEA in dual mode. The device in platinum nanoparticles (Pt NPs) loaded on an octahedral cuprous oxide (Cu 2 O) surface has excellent peroxidase performance. Using Cu 2 O/Pt NPs as a signal tag can not only generate a larger response current in electrochemical mode but also effectively catalyze 3,3′,5,5′-tetramethyl benzidine (TMB) color development in colorimetric mode. The results show that the dual mode sensor has good detection performance. Using the electrochemical analysis method, the detection range was 0.1 pg/mL - 80 ng/mL, and the detection limit was 0.03 pg/mL. The detection range of colorimetric analysis technology was 0.1 ng/mL - 80 ng/mL, and the detection limit was 0.026 ng/mL. Therefore, the dual-mode sensor has excellent detection performance, good selectivity, reproducibility and stability and provides a new detection method for early cancer detection and prognosis monitoring.

研究领域: 生物医学工程 · 分析化学 · 癌症诊断
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Plasmonics · 2015 ·Vol. 11 ·期 2 ·565-572 · IF 2.238

Tuning the Fluorescence Quenching Properties of Plasmonic Ag-Coated-Au Triangular Nanoplates: Application in Ultrasensitive Detection of CEA

Zhu Jian,Wang Jing-Fei,Li Jian-Jun,Zhao Jun-Wu

By using the fluorescence spectroscopic techniques, the fluorescence quenching abilities of gold triangular nanoplates with silver coating have been studied. Because of the surface plasmon resonance (SPR)-induced nonradiative energy transformation, the fluorescence emission intensity of carcinoembryonic antigen (CEA) could be greatly quenched by the silver-coated-gold triangular nanoplates. By comparing with the bare gold triangular nanoplates, the nanoplates with silver coating exhibit greater fluorescence quenching ability and could be further improved by increasing the coating thickness. The fluorescence quenching effect also depends on the concentration of CEA. For bare gold triangular nanoplates, the quenching ability to CEA is decreased as the CEA concentration is increased. Whereas for silver-coated-gold triangular nanoplates, the quenching ability to CEA is increased as the CEA concentration is increased. By analyzing the intensity quenching of the fluorescence peak, CEA could be detected with an ultra-low detection limit of 5 pg/mL.

研究领域: 生物医学 · 纳米技术 · 光学检测
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TALANTA · 2022 · IF 6.556

Molybdenum blue mediated photothermal immunoassay for CEA detection based on Ag4P2O7@Ag nanocomposites

Yanfei Wen,Yuan Yuan,Bing Zhang,Jianying Lin,Zhihuan Zhao,Jing Li,Yan Cheng

A photothermal immunoassay was built for tumor marker detection based on Ag 4 P 2 O 7 @Ag nanocomposites. Ag 4 P 2 O 7 @Ag nanomaterials were synthesized by precipitation-photoreduction reaction, and characterized by transmission electron microscope (TEM), scanning electron microscopy (SEM), atomic force microscopy (AFM), X-ray photoelectron spectra (XPS) and X-ray powder diffraction (XRD). Come about PO 4 3− derived from Ag 4 P 2 O 7 @Ag under acidic conditions react with ammonium molybdate in the action of reductant generating molybdenum blue. The photothermal change is due to molybdenum blue solution depending on the concentration of carcinoembryonic antigen (CEA) in immunoassay. Under optimal conditions, there is a linear relation between ΔT and CEA concentration in the range of 1 pg mL −1 –40 ng mL −1 with the detection limit of 0.33 pg mL −1 . Meanwhile, the developed photothermal immunoassay displays preferable selectivity , repeatability, and stability.

研究领域: 分析化学 · 纳米技术 · 癌症研究
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